Epoxidation of styrene by anhydrous t-butyl hydroperoxide over gold supported on Al2O3, Ga2O3, In2O3 and Tl2O3

被引:87
作者
Patil, NS
Jha, R
Uphade, BS
Bhargava, SK
Choudhary, VR [1 ]
机构
[1] Natl Chem Lab, Chem Engn & Proc Dev Div, Pune 411008, Maharashtra, India
[2] RMIT Univ, Dept Appl Chem, Melbourne, Vic 3000, Australia
关键词
epoxidation of styrene; styrene oxide; t-butyl hydroperoxide; gold supported on Gr. IIIa metal oxides;
D O I
10.1016/j.apcata.2004.07.023
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Group IIIa metal (viz. Al, Ga, In and Tl) oxide-supported gold nanoparticles, prepared by deposition-precipitation (DP) using NaOH and by homogeneous deposition-precipitation (HDP) using urea, were employed as highly active/selective and reusable catalysts for the epoxidation of styrene (at 82 degreesC) by anhydrous t-butyl hydroperoxide (TBHP). The loading and average particle size of gold, when it was deposited on the Gr. IIIa metal oxides by the HDP, was found to increase in the following order: Al2O3 (6.36 wt.%, 4.1 +/- 2.3 nm) < Ga2O3 (6.43 wt.%, 6.67 +/- 3.7 nm) < In2O3 (6.81 wt.%, 15.6 +/- 6.3 nm) < Tl2O3 (8.00 wt.%, 24.4 +/- 13.1 nm). Both the activity and the epoxide selectivity of the supported gold catalysts are in the following order: Au/Al2O3 < Au/Ga2O3 < Au/In2O3 < Au/Tl2O3. Using the DP method, the Au loading on Al2O3 and Tl2O3 was found to be 2.10 and 5.42 wt.%, respectively, such values are much lower than those achieved by the HDP method. The Al2O3, Ga2O3 and In2O3 supports alone showed little or no epoxidation activity/selectivity. However, the Tl2O3 support alone showed the activity and epoxide selectivity comparable to that of the Au/Tl2O3 Catalysts. The surface species on the Au/Al2O3 were found to be only metallic gold (Au-0) ones and Al in single oxidation state (Al3+). However, the surface species on the Au/In2O3 were both the metallic and ionic gold (Au-0 and Au3+) and the indium in two oxidation states (In3+ and In2+ or In1+). The gold loading and both the epoxidation activity and selectivity are increased with increasing the basicity and/or reduction potential of the support used in the supported Au catalysts. (C) 2004 Elsevier B.V. All rights reserved.
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页码:87 / 93
页数:7
相关论文
共 26 条
[11]   Epoxidation of styrene by anhydrous t-butyl hydroperoxide over Au/TiO2 catalysts [J].
Patil, NS ;
Uphade, BS ;
Jana, P ;
Sonawane, RS ;
Bhargava, SK ;
Choudhary, VR .
CATALYSIS LETTERS, 2004, 94 (1-2) :89-93
[12]   Activation of Au nanoparticles on oxide surfaces:: reaction of SO2 with Au/MgO(100) [J].
Rodriguez, JA ;
Pérez, M ;
Jirsak, T ;
Evans, J ;
Hrbek, J ;
González, L .
CHEMICAL PHYSICS LETTERS, 2003, 378 (5-6) :526-532
[13]   Synergism in methanol synthesis from carbon dioxide over gold catalysts supported on metal oxides [J].
Sakurai, H ;
Haruta, M .
CATALYSIS TODAY, 1996, 29 (1-4) :361-365
[14]  
STRANGLAND EE, 2000, J CATAL, V199, P332
[15]  
Swern D., 1971, ORGANIC PEROXIDE, V2
[16]  
TANABE K, 1969, PREPARATION CATALYST, V1, P65
[17]  
TSUBOTA S, 1991, STUD SURF SCI CATAL, V63, P695
[18]   Selective oxidation of propylene to propylene oxide or propionaldehyde over Au supported on titanosilicates in the presence of H2 and O2 [J].
Uphade, BS ;
Tsubota, S ;
Hayashi, T ;
Haruta, M .
CHEMISTRY LETTERS, 1998, (12) :1277-1278
[19]   Vapor-phase epoxidation of propene using H2 and O2 over Au/Ti-MCM-48 [J].
Uphade, BS ;
Akita, T ;
Nakamura, T ;
Haruta, M .
JOURNAL OF CATALYSIS, 2002, 209 (02) :331-340
[20]   Surface modified amorphous titanosilicate catalysts for liquid phase epoxidation [J].
Van Grieken, R ;
Sotelo, JL ;
Martos, C ;
Fierro, JLG ;
López-Granados, M ;
Mariscal, R .
CATALYSIS TODAY, 2000, 61 (1-4) :49-54